Habilitations from 2018

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Jaekel, Konrad; Sauni Camposano, Yesenia Haydee; Matthes, Sebastian; Glaser, Marcus; Schaaf, Peter; Bergmann, Jean Pierre; Müller, Jens; Bartsch, Heike
Ni/Al multilayer reactions on nanostructured silicon substrates. - In: Journal of materials science, ISSN 1573-4803, Bd. 58 (2023), 31, S. 12811-12826

Fast energy release, which is a fundamental property of reactive multilayer systems, can be used in a wide field of applications. For most applications, a self-propagating reaction and adhesion between the multilayers and substrate are necessary. In this work, a distinct approach for achieving self-propagating reactions and adhesion between deposited Ni/Al reactive multilayers and silicon substrate is demonstrated. The silicon surface consists of random structures, referred to as silicon grass, which were created by deep reactive ion etching. Using the etching process, structure units of heights between 8 and 13 µm and density between 0.5 and 3.5 structures per µm^2 were formed. Ni and Al layers were alternatingly deposited in the stoichiometric ratio of 1:1 using sputtering, to achieve a total thickness of 5 µm. The analysis of the reaction and phase transformation was done with high-speed camera, high-speed pyrometer, and X-ray diffractometer. Cross-sectional analysis showed that the multilayers grew only on top of the silicon grass in the form of inversed cones, which enabled adhesion between the silicon grass and the reacted multilayers. A self-propagating reaction on silicon grass was achieved, due to the thermally isolating air pockets present around these multilayer cones. The velocity and temperature of the reaction varied according to the structure morphology. The reaction parameters decreased with increasing height and decreasing density of the structures. To analyze the exact influence of the morphology, further investigations are needed.

Wöste, Andreas; Hergert, Germann; Quenzel, Thomas; Silies, Martin; Wang, Dong; Groß, Petra; Lienau, Christoph
Ultrafast coupling of optical near fields to low-energy electrons probed in a point-projection microscope. - In: Nano letters, ISSN 1530-6992, Bd. 23 (2023), 12, S. 5528-5534

We report the first observation of the coupling of strong optical near fields to wavepackets of free, 100 eV electrons with <50 fs temporal resolution in an ultrafast point-projection microscope. Optical near fields are created by excitation of a thin, nanometer-sized Yagi-Uda antenna, with 20 fs near-infrared laser pulses. Phase matching between electrons and near fields is achieved due to strong spatial confinement of the antenna near field. Energy-resolved projection images of the antenna are recorded in an optical pump-electron probe scheme. We show that the phase modulation of the electron by transverse-field components results in a transient electron deflection while longitudinal near-field components broaden the kinetic energy distribution. This low-energy electron near-field coupling is used here to characterize the chirp of the ultrafast electron wavepackets, acquired upon propagation from the electron emitter to the sample. Our results bring direct mapping of different vectorial components of highly localized optical near fields into reach.

Matthes, Sebastian; Glaser, Marcus; Vardo, Emina; Sauni Camposano, Yesenia Haydee; Jaekel, Konrad; Bergmann, Jean Pierre; Schaaf, Peter
Influence of extrinsic induced tensile stress on the self-propagating high-temperature synthesis of nanosized Al/Ni multilayers. - In: Journal of materials science, ISSN 1573-4803, Bd. 58 (2023), 24, S. 10085-10095

Reactive multilayer systems consisting of alternating nanoscale Al and Ni layers are applicable in joining, various pyrotechnic applications and thermal batteries. Since diffusion based high-temperature synthesis occurs without the presence of air, efforts have focused on investigating the understanding of the fundamental reaction processes and characteristics. The aim of this study is to expose the reactive multilayers to extrinsic induced tensile stress so that the self-propagating synthesis can proceed under these conditions. Further, the properties during and after the reaction will be investigated. Multilayers deposited by sputtering on Kapton® substrates with different bilayer- and total thicknesses as well as commercial Nanofoils® with thicknesses of 40 µm and 60 µm were used as samples. The investigations focused on the propagation velocity measured with a high-speed camera, the temperature regime determined with a high-speed pyrometer, and the formed phases after the synthesis examined via X-ray diffraction. The gained results of this study reveal important insights for the application of the reactive Al/Ni multilayer system in terms of stability or reliability related to propagation front velocity, maximum temperature and formed phases under induced external tensile stresses.

Isaac, Nishchay Angel; Schlag, Leslie; Ispas, Adriana; Reiprich, Johannes; Soydan, Alper K.; Moreira, Pedro H. O.; Thiele, Sebastian; Aliabadian, Bardia; Flock, Dominik; Knauer, Andrea; Jiménez, Juan J.; Bund, Andreas; Morales Sánchez, Francisco Miguel; Pezoldt, Jörg; Jacobs, Heiko O.
Novel gas phase route toward patterned deposition of sputter-free Pt/Al nanofoils. - In: Advanced Materials Technologies, ISSN 2365-709X, Bd. 0 (2023), 0, 2300448, S. 1-8

This article reports a new approach toward fabrication and directed assembly of nanoparticulate reactive system (Nanofoils) on patterned substrates. Different from current state-of-the-art, gas phase electrodeposition uses nanoparticles instead of atoms to form densely packed multilayered thin films at room temperature-pressure. On ignition, the multilayer system undergoes an exothermic self-propagating reaction. The numerous contact points between two metallic nanoparticulate layers aid in high heat release. Sub-10-nm Platinum (Pt) and Aluminum (Al) particles are synthesized through cathode erosion of metal electrodes in a flow of pure nitrogen gas (spark ablation). Pt/Al bilayer stacks with total thickness of 3-8 µm undergo self-propagating reaction with a 10.3 mm s^−1 wavefront velocity on local ignition. The reaction wavefront is captured using high speed videography. Calorimetry studies reveal two exothermic peaks suggesting Pt/Al alloy formation. The peak at 135 &ring;C has a higher calorific value of 150 mW g^−1 while the peak at 400 &ring;C has a 12 mW g^−1 exothermic peak. X-ray diffraction study shows reaction-products are cubic Al2Pt with small quantities of orthorhombic Al6Pt and orthorhombic AlPt2. Electron microscopy studies help draw a correlation between film morphology, bimetallic interface, nanoparticle oxidation, and self-propagating reaction kinetics that is significant in broadening our understanding towards nanoparticulate reactive systems.

Heiniger-Schell, Juliana; Bharuth-Ram, Krish; Naicker, Kimara; Masondo, Vusumuzi; Dang, Thien Thanh; Escobar Castillo, Marianela; Díaz-Guerra, Carlos; Marschick, Georg; Masenda, Hilary; Gunnlaugsson, Haraldur P.; Qi, Bingcui; Unzueta, Iraultza; Ólafsson, Sveinn; Adhikari, Rajdeep; Peters, Gerrard; Naidoo, Deena; Schaaf, Peter; Zyabkin, Dmitry; Johnston, Karl; Becker, Sven; Jakob, Gerhard
Temperature dependence of the hyperfine magnetic field at Fe sites in Ba-doped BiFeO3 thin films studied by emission Mössbauer spectroscopy. - In: Crystals, ISSN 2073-4352, Bd. 13 (2023), 5, 724, S. 1-13

Emission 57Fe Mössbauer spectroscopy (eMS), following the implantation of radioactive 57Mn+ ions, has been used to study the temperature dependence of the hyperfine magnetic field at Fe sites in Ba-doped BiFeO3 (BFO) thin films. 57Mn β decays (t1/2 = 90 s) to the 14.4 keV Mössbauer state of 57Fe, thus allowing online eMS measurements at a selection of sample temperatures during Mn implantation. The eMS measurements were performed on two thin film BFO samples, 88 nm and 300 nm thick, and doped to 15% with Ba ions. The samples were prepared by pulsed laser deposition on SrTiO3 substrates. X-ray diffraction analyses of the samples showed that the films grew in a tetragonal distorted structure. The Mössbauer spectra of the two films, measured at absorber temperatures in the range 301 K-700 K, comprised a central pair of paramagnetic doublets and a magnetic sextet feature in the wings. The magnetic component was resolved into (i) a component attributed to hyperfine interactions at Fe3+ ions located in octahedral sites (Bhf); and (ii) to Fe3+ ions in implantation induced lattice defects, which were characterized by a distribution of the magnetic field BDistr. The hyperfine magnetic field at the Fe probes in the octahedral site has a room temperature value of Bhf = 44.5(9) T. At higher sample temperatures, the Bhf becomes much weaker, with the Fe3+ hyperfine magnetic contribution disappearing above 700 K. Simultaneous analysis of the Ba-BFO eMS spectra shows that the variation of the hyperfine field with temperature follows the Brillouin curve for S = 5/2.

Li, Feitao; Flock, Dominik; Wang, Dong; Schaaf, Peter
Solid-state dewetting of Ag/Ni bi-layers: accelerated void formation by the stress gradient in the bottom Ni layer. - In: Journal of alloys and compounds, Bd. 960 (2023), 170735

Solid-state dewetting (SSD) of the immiscible Ag/Ni bi-layers was studied. After annealing at 400 &ring;C for 1 min, the Ag film was dewetted on the Ni film, and this is the first observation about the SSD of one metal film on another metal film. The easier dewetting of Ag than Ni was attributed to its lower melting point, faster grain boundary self-diffusion and poor wettability between them. At 500 &ring;C, the void formation in the bottom Ni layer was highlighted and compared to Ni single layer: many voids in the former while no visible voids in the latter, indicating that the presence of Ag accelerated the SSD of Ni. It was attributed to the vertical stress gradient in the bottom Ni film of Ag/Ni bi-layers, which accelerated the Ni diffusion and formation of the voids in the underlying Ni film around and below the Ag particles. Besides, voids were more easily formed below the Ag particles than between them due to the large lattice mismatch at the Ag/Ni interface and the possible formation of Ag-Ni alloys. The destabilization of the Ag on the Ni film contributes to the understanding of dewetting kinetics, which is beneficial to realize the controllable nanofabrication.

Mathew, Sobin; Reiprich, Johannes; Narasimha, Shilpashree; Abedin, Saadman; Kurtash, Vladislav; Thiele, Sebastian; Hähnlein, Bernd; Scheler, Theresa; Flock, Dominik; Jacobs, Heiko O.; Pezoldt, Jörg
Three-dimensional MoS2 nanosheet structures: CVD synthesis, characterization, and electrical properties. - In: Crystals, ISSN 2073-4352, Bd. 13 (2023), 3, 448, S. 1-14

The proposed study demonstrates a single-step CVD method for synthesizing three-dimensional vertical MoS2 nanosheets. The postulated synthesizing approach employs a temperature ramp with a continuous N2 gas flow during the deposition process. The distinctive signals of MoS2 were revealed via Raman spectroscopy study, and the substantial frequency difference in the characteristic signals supported the bulk nature of the synthesized material. Additionally, XRD measurements sustained the material’s crystallinity and its 2H-MoS2 nature. The FIB cross-sectional analysis provided information on the origin and evolution of the vertical MoS2 structures and their growth mechanisms. The strain energy produced by the compression between MoS2 islands is assumed to primarily drive the formation of vertical MoS2 nanosheets. In addition, vertical MoS2 structures that emerge from micro fissures (cracks) on individual MoS2 islands were observed and examined. For the evaluation of electrical properties, field-effect transistor structures were fabricated on the synthesized material employing standard semiconductor technology. The lateral back-gated field-effect transistors fabricated on the synthesized material showed an n-type behavior with field-effect mobility of 1.46 cm2 V^-1 s^-1 and an estimated carrier concentration of 4.5 × 10^12 cm^-2. Furthermore, the effects of a back-gate voltage bias and channel dimensions on the hysteresis effect of FET devices were investigated and quantified.

Li, Feitao; Wan, Siyao; Wang, Dong; Schaaf, Peter
Formation of nanoflowers: Au and Ni silicide cores surrounded by SiOx branches. - In: Beilstein journal of nanotechnology, ISSN 2190-4286, Bd. 14 (2023), 1, S. 133-140

This work reports the formation of nanoflowers after annealing of Au/Ni bilayers deposited on SiO2/Si substrates. The cores of the nanoflowers consist of segregated Ni silicide and Au parts and are surrounded by SiOx branches. The SiO2 decomposition is activated at 1050 &ring;C in a reducing atmosphere, and it can be enhanced more by Au compared to Ni. SiO gas from the decomposition of SiO2 and the active oxidation of Si is the source of Si for the growth of the SiOx branches of the nanoflowers. The concentration of SiO gas around the decomposition cavities is inhomogeneously distributed. Closer to the cavity border, the concentration of the Si sources is higher, and SiOx branches grow faster. Hence, nanoflowers present shorter and shorter branches as they are getting away from the border. However, such inhomogeneous SiO gas concentration is weakened in the sample with the highest Au concentration due to the strong ability of Au to enhance SiO2 decomposition, and nanoflowers with less difference in their branches can be observed across the whole sample.

Grunert, Malte; Bohm, Sebastian; Honig, Hauke; Wang, Dong; Lienau, Christoph; Runge, Erich; Schaaf, Peter
Structural and optical properties of gold nanosponges revealed via 3D nano-reconstruction and phase-field models. - In: Communications materials, ISSN 2662-4443, Bd. 4 (2023), 1, 20, S. 1-13

Nanosponges are subject of intensive research due to their unique morphology, which leads among other effects to electrodynamic field localization generating a strongly nonlinear optical response at hot spots and thus enable a variety of applications. Accurate predictions of physical properties require detailed knowledge of the sponges’ chaotic nanometer-sized structure, posing a metrological challenge. A major goal is to obtain computer models with equivalent structural and optical properties. Here, to understand the sponges’ morphology, we present a procedure for their accurate 3D reconstruction using focused ion beam tomography. Additionally, we introduce a simulation method to create nanoporous sponge models with adjustable geometric properties. It is shown that if certain morphological parameters are similar for computer-generated and experimental sponges, their optical response, including magnitudes and hot spot locations, are also similar. Finally, we analyze the anisotropy of experimental sponges and present an easy-to-use method to reproduce arbitrary anisotropies in computer-generated sponges.

Cheng, Pengfei; Wang, Dong
Easily repairable and high-performance carbon nanostructure absorber for solar photothermoelectric conversion and photothermal water evaporation. - In: ACS applied materials & interfaces, ISSN 1944-8252, Bd. 15 (2023), 6, S. 8761-8769

Carbon materials are a category of broadband solar energy harvesting materials that can convert solar energy into heat under irradiation, which can be used for photothermal water evaporation and photothermoelectric power generation. However, destruction of the carbon nanostructure during usage will significantly decrease the light-trapping performance and, thus, limit their practical applications. In this article, an easily repairable carbon nanostructure absorber with full-solar-spectrum absorption and a hierarchically porous structure is prepared. The carbon absorber shows a superhigh light absorption of above 97% across the whole solar spectrum because of multiple scatterings within the carbon nanostructure and photon interaction with the carbon nanoparticles. The excellent light absorption performance directly leads to a good photothermal effect. As a consequence, the carbon absorber integrated with a thermoelectric module can obtain a large power (133.3 μW cm-2) output under 1 sun. In addition, the carbon absorber combined with the sponge can achieve a high photothermal water evaporation efficiency of 83.6% under 1 sun. Its high-efficiency solar-to-electricity and photothermal water evaporation capabilities demonstrate that the carbon absorber with superhigh absorption, simple fabrication, and facile repairability shows great potential for practical fresh water production and electric power generation.